The effect of oxygen concentration on the speciation of laser ablated uranium
Abstract In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that betw...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2022-03-01
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| Series: | Scientific Reports |
| Online Access: | https://doi.org/10.1038/s41598-022-07834-9 |
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| author | Mark A. Burton Alex W. Auner Jonathan C. Crowhurst Peter S. Boone Lauren A. Finney David G. Weisz Batikan Koroglu Igor Jovanovic Harry B. Radousky Kim B. Knight |
| author_facet | Mark A. Burton Alex W. Auner Jonathan C. Crowhurst Peter S. Boone Lauren A. Finney David G. Weisz Batikan Koroglu Igor Jovanovic Harry B. Radousky Kim B. Knight |
| author_sort | Mark A. Burton |
| collection | DOAJ |
| description | Abstract In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either 16O2 or 18O2, to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UOx (am-UOx, where 3 ≤ x ≤ 4) and UO2 after ablation in 1 atm of pure O2 and a 1% O2/Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O2 suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UOx and UO2 particulates convert to α-U3O8 when heated. Lastly, experiments performed in 18O2 environments show the formation of 18O-substituted uranium oxides; vibrational frequencies for am-U18Ox are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator can be used in current models of nuclear explosions to improve our predicative capabilities of chemical speciation. |
| first_indexed | 2024-12-23T13:09:37Z |
| format | Article |
| id | doaj.art-3c31b35e7d544f5793db7eac7d37fce6 |
| institution | Directory Open Access Journal |
| issn | 2045-2322 |
| language | English |
| last_indexed | 2024-12-23T13:09:37Z |
| publishDate | 2022-03-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Scientific Reports |
| spelling | doaj.art-3c31b35e7d544f5793db7eac7d37fce62022-12-21T17:45:46ZengNature PortfolioScientific Reports2045-23222022-03-0112111110.1038/s41598-022-07834-9The effect of oxygen concentration on the speciation of laser ablated uraniumMark A. Burton0Alex W. Auner1Jonathan C. Crowhurst2Peter S. Boone3Lauren A. Finney4David G. Weisz5Batikan Koroglu6Igor Jovanovic7Harry B. Radousky8Kim B. Knight9Lawrence Livermore National LaboratoryLawrence Livermore National LaboratoryLawrence Livermore National LaboratoryLawrence Livermore National LaboratoryDepartment of Nuclear Engineering and Radiological Sciences, University of MichiganLawrence Livermore National LaboratoryLawrence Livermore National LaboratoryDepartment of Nuclear Engineering and Radiological Sciences, University of MichiganLawrence Livermore National LaboratoryLawrence Livermore National LaboratoryAbstract In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either 16O2 or 18O2, to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UOx (am-UOx, where 3 ≤ x ≤ 4) and UO2 after ablation in 1 atm of pure O2 and a 1% O2/Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O2 suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UOx and UO2 particulates convert to α-U3O8 when heated. Lastly, experiments performed in 18O2 environments show the formation of 18O-substituted uranium oxides; vibrational frequencies for am-U18Ox are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator can be used in current models of nuclear explosions to improve our predicative capabilities of chemical speciation.https://doi.org/10.1038/s41598-022-07834-9 |
| spellingShingle | Mark A. Burton Alex W. Auner Jonathan C. Crowhurst Peter S. Boone Lauren A. Finney David G. Weisz Batikan Koroglu Igor Jovanovic Harry B. Radousky Kim B. Knight The effect of oxygen concentration on the speciation of laser ablated uranium Scientific Reports |
| title | The effect of oxygen concentration on the speciation of laser ablated uranium |
| title_full | The effect of oxygen concentration on the speciation of laser ablated uranium |
| title_fullStr | The effect of oxygen concentration on the speciation of laser ablated uranium |
| title_full_unstemmed | The effect of oxygen concentration on the speciation of laser ablated uranium |
| title_short | The effect of oxygen concentration on the speciation of laser ablated uranium |
| title_sort | effect of oxygen concentration on the speciation of laser ablated uranium |
| url | https://doi.org/10.1038/s41598-022-07834-9 |
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